The development of low-cost, efficient catalysts for electrocatalytic water splitting to generate green hydrogen is a hot topic among researchers. Herein, we have developed a highly efficient heterostructure of CoCr-LDH on NiO on nickel foam (NF) for the first time. The preparation strategy follows the simple annealing of a cleaned NF without using any Ni salt precursor, followed by the growth of CoCr-LDH nanosheets over the surface-oxidized NF. The CoCr-LDH/NiO/NF catalyst shows excellent electrocatalytic activity and stability toward oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in a 1 M KOH solution. For OER, only 253 mV and for HER, only 185 mV overpotentials are required to attain a 50 mA cm